ZnO thin films were prepared on Si(111) substrates by pulsed laser deposition (PLD). Then, the samples were annealed at different temperatures in NH 3 ambient and their properties were investigated particularly as a function of annealing temperature. The structure, morphology, and optical properties of ZnO films were studied by x-ray diffraction (XRD), Fourier transform infrared spectroscope (FTIR), scanning electron microscope (SEM), and photoluminescence (PL). The results show that the increase of annealing temperature makes for the improvement in the crystal quality and surface morphology below the temperature of 650°C. However, when the annealing temperature is above 650°C, the ZnO films will volatilize and, especially at 750°C, ZnO will volatilize completely.